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Article history: The phenomenon of ultraviolet (UV) radiation aging gradient in asphalt binder is existent but usually
Received 7 October 2019 neglected in most of UV radiation aging simulations and real asphalt pavement. Therefore, it is necessary
Received in revised form 21 December 2019 to investigate the developing velocity and causing mechanism of UV aging gradient in asphalt binder. In
Accepted 17 February 2020
this paper, the 3 mm-thickness asphalt films that suffered different UV radiation aging periods were
Available online 25 February 2020
divided into average three layers by peeling procedures. Then, rheological properties, molecular sizes dis-
tributions, chemical functional groups contents and fluorescence tests were conducted on different
Keywords:
asphalt layers. The results indicate that by rheological indexes, the effect of 6-day UV aging is almost neg-
Asphalt binder
Ultraviolet radiation aging
ligible, but the UV aging depth can exceed 1 mm after 9-day UV aging period and further exceed 2 mm
Aging gradient after 15-day UV aging period. In addition, the vertical gradients of molecular sizes and oxidation products
Rheological indexes contents tend to form in asphalt film as UV aging process proceeds. Moreover, the observation of inor-
Diffusion aging model ganic fluorescent powders being able to permeate into fresh asphalt film in lower layers by fluorescence
microscope objectively demonstrates the ‘‘diffusion aging model” ─ UV aged asphalt molecules diffuse
downwards into fresh asphalt film in lower layer.
Ó 2020 Elsevier Ltd. All rights reserved.
https://doi.org/10.1016/j.conbuildmat.2020.118501
0950-0618/Ó 2020 Elsevier Ltd. All rights reserved.
2 Z. Chen et al. / Construction and Building Materials 246 (2020) 118501
Table 1
Basic properties of base asphalt.
Frequency sweep tests from 0.1 to 100 rad/s were performed Based on principle of GPC test, asphalt molecules with different
by dynamic shear rheometer (DSR) in strain-controlled mode. sizes can be sequentially separated with the elution time increas-
The sweep temperatures were controlled at 60 °C and 5 °C ing. Specifically, molecules with larger molecular size are eluted
respectively, and the 25 mm spindle and 8 mm spindle were cor- out earlier. In order to quantitatively describe the asphalt molecu-
respondingly selected [24]. Based on amplitude sweep results, 1% lar size distributions, the chromatographic profile is divided into
strain amplitude was chosen to make asphalt rheological behav- average 13 slices in terms of elution time, as illustrated in Fig. 4.
ior within linear viscoelastic (LVE) range. Values of complex mod- The ratio value of integral area of chromatographic curve within
ulus at 60 °C and phase angle at 5 °C were collected from 1–5 slices to whole integral area within 1–13 slices is defined as
frequency sweep to evaluate rheological properties at different large molecular size (LMS) that indicates the proportion of mole-
temperatures. cules with large size. By analogy, the ratio values of integral areas
It is known that zero shear viscosity (ZSV) is an indicator that within 6–9 slices and 10–13 slices to whole integral area corre-
can be used to evaluate the high-temperature rutting resistance spond to medium molecular size (MMS) and small molecular size
of asphalt binder [25,26]. The value of ZSV at 60 °C can be calcu- (SMS), respectively [34–36].
lated by fitting the complex viscosity versus frequency curve with
simplified Cross model [5]. In addition, multiple stress creep recov-
ery (MSCR) tests at 60 °C were conducted in accordance with ASTM 2.6. Fourier transform infrared spectroscopy (FTIR) test
D7405, and non-recoverable creep compliance (Jnr) values at differ-
ent stress levels (0.1 and 3.2 kPa) were calculated to evaluate the It is demonstrated that carbonyl and sulfoxide groups are main
asphalt rutting resistance as well [27,28]. oxidation products of asphalt binder [37–39]. Thus, the UV aging
The DSR function (DSRFn) index has been demonstrated to
correlate well with cracking resistance of asphalt pavement
[29–31]. Its definition is shown as formula (1). It is a calculated
value at a specific time–temperature condition ─ the tempera-
ture of 15 °C and the frequency of 0.005 rad/s. The specific calcu-
lation procedures of DSRFn index can be referred to previously
published papers [5]. The crossover frequency (xc) is the value
at which the storage modulus is equal to the loss modulus or
the phase angle is equal to 45° during frequency sweep. xc can
reflect the overall hardness of asphalt binder, and the smaller
xc at low temperatures manifests the more brittle asphalt binder
[32,33]. In this paper, xc values were obtained from frequency
sweep at 5 °C.
G0
DSRFn ¼ g0 ð1Þ
G0
where
degree of different asphalt layers can be evaluated by contents of The scanning spectra from 400 to 4000 cm1 were recorded
these functional groups. Carbonyl and sulfoxide indexes are with a resolution of 4 cm1 and scanning times of 32.
defined by formula (2) and (3), respectively.
2.7. Fluorescence test
A1700
CI ¼ P ð2Þ
A In order to demonstrate the ‘‘diffusion aging model”, inorganic
fluorescent powders with size of 1–10 lm were utilized as tracer
A1030 to be added into the top 1 mm-thickness asphalt layer, as shown
SI ¼ P ð3Þ
A in Fig. 5. After 15-day UV aging period, the middle and bottom
asphalt layers were observed by two-photon confocal microscopy
P
where A is equal to total areas of peaks centered around with 60 times objective lens to detect whether fluorescence reac-
1700 cm1, 1600 cm1, 1460 cm1, 1376 cm1, 1030 cm1, tion can occur. As control sample, the un-UV aged 3 mm-
864 cm1, 814 cm1, 743 cm1, 724 cm1. A1700 and A1030 corre- thickness asphalt film whose top layer also contained inorganic
spond to characteristic peak areas of carbonyl and sulfoxide groups, fluorescent powders was stored at 50 °C for 15 days to prove
respectively. whether fluorescent powders will diffuse downwards without UV
radiation influence. Three replicates were used for each asphalt
sample in fluorescence test.
Fig. 6. Complex moduli at 60 °C for different layers in UV aged asphalt samples that suffer different UV aging periods: (a) UV aging 6 days, (b) UV aging 9 days, (c) UV aging
12 days, and (d) UV aging 15 days.
Z. Chen et al. / Construction and Building Materials 246 (2020) 118501 5
deformation. Generally, the stiffer asphalt binder exhibits the lar- the UV radiation aging time lasts 15 days, and there is an obvious
ger complex modulus. Fig. 6 presents complex moduli at 60 °C vertical gradient of rheological properties in 3 mm-thickness
for different layers in UV aged asphalt samples that suffer different asphalt film at this time. Based on above results, it can be con-
UV aging periods. It can be seen in Fig. 6(a) that when the UV aging cluded that the UV aging depth gradually expands downwards as
period lasts only 6 days, there are almost no obvious differences of the UV aging time increases.
complex moduli among the top, middle and bottom asphalt layers, The asphalt binder is a viscoelastic material, and the index of
and complex moduli of these layers are all similar to value of orig- phase angle can reflect the proportion of viscous component to
inal sample. It is suggested that the effects of 6-day UV radiation elastic component. At low temperatures, the asphalt binder with
aging do not cause the gradient of rheological properties in the larger phase angle possesses the stronger viscous mobility
3 mm-thickness asphalt film. After UV radiation aging 9 days, com- and more potential to resist the cracking damage. Phase angle val-
plex moduli of the top and middle asphalt layers start to increase, ues at 5 °C for different layers in UV aged asphalt samples that suf-
especially for the top asphalt layer. But the complex modulus of fer different UV aging periods are shown in Fig. 7. It is interesting
bottom asphalt layer is still not remarkably different from value that the evolutions of UV aging depth in asphalt binder reflected by
of original asphalt binder, illustrating the depth influenced by UV phase angle are entirely consistent with results obtained from
radiation aging is only within 2 mm. The effects of 12-day UV radi- complex modulus. In addition, with the aging time increasing,
ation aging only further raise the complex moduli of the top and the phase angle value of the same asphalt layer gradually
middle asphalt layers, but the bottom asphalt layer is not yet influ- decreases, which indicates the UV aging increases the elastic
enced by UV radiation aging, as shown in Fig. 6(c). Until UV radia- response of asphalt binder and makes it stiffer and more brittle.
tion aging time extends to 15 days, complex moduli of the top,
middle and bottom asphalt layers are all larger than that of original
asphalt binder, and from bottom layer to top layer, the value of 3.1.2. ZSV and Jnr
complex modulus gradually increases. These demonstrate that The UV aging destructs the balance of asphalt colloidal struc-
the depth influenced by UV radiation aging exceeds 2 mm when ture by changing the chemical components of asphalt binder,
Fig. 7. Phase angle values at 5 °C for different layers in UV aged asphalt samples that suffer different UV aging periods: (a) UV aging 6 days, (b) UV aging 9 days, (c) UV aging
12 days, and (d) UV aging 15 days.
6 Z. Chen et al. / Construction and Building Materials 246 (2020) 118501
Fig. 10. DSRFn values of different layers in UV aged asphalt samples that suffer
Fig. 8. ZSV values of different layers in UV aged asphalt samples that suffer
different UV aging periods.
different UV aging periods.
Fig. 9. Jnr values of different layers in UV aged asphalt samples that suffer different UV aging periods: (a) Jnr at 0.1 kPa and (b) Jnr at 3.2 kPa.
Z. Chen et al. / Construction and Building Materials 246 (2020) 118501 7
and xc values of different layers in UV aged asphalt samples that sizes will change from smaller ones towards larger ones as aging
suffer different UV aging periods are illustrated in Figs. 10 and processes proceed [34–36].
11, respectively. The results reflected by DSRFn and xc are almost The results of molecular size distributions in different layers of
entirely consistent with those reflected by complex modulus, 15-day UV aged asphalt sample are presented in Table 2. Compared
phase angle, ZSV and Jnr. It is demonstrated that the UV aging with original sample, the 15-day UV aged asphalt sample exhibits
can cause a gradient distribution of brittleness in asphalt films. larger LMS and smaller SMS values no matter what asphalt layer is.
This means every asphalt layer is influenced after 15-day UV aging
3.2. Analyses by GPC period, which is consistent with results reflected by rheological
indexes. In addition, as the vertical position of asphalt layer deep-
The change of chemical components is one of the characteristics ens, the LMS value gradually declines but the SMS value displays a
during aging processes of asphalt binder. Generally, the proportion contrary trend, demonstrating the existence of vertical gradient of
of light components with small molecular sizes is decreased while molecular size distributions in 3-mm thickness asphalt film after
the share of heavy components with large molecular sizes is 15-day UV aging period.
increased due to the volatilization and association reactions. Corre- The UV radiation can only penetrate through about 4.5 lm-
spondingly, in terms of molecular size distributions, molecular thickness asphalt film. In another words, merely the 4.5 lm-
thickness asphalt film can be directly influenced by UV radiation
Table 2 [17]. However, it is investigated that with the aging period extend-
The results of molecular size distributions. ing, the UV radiation aging depth is able to greatly exceed this
value to a few millimeters or even more. Zeng et al. [17] explained
Asphalt binders LMS (%) MMS (%) SMS (%)
that UV aged asphalt molecules with relatively large sizes diffuse
Origin 15.75 61.84 22.41
downwards into fresh asphalt film in lower layer, which conse-
15–1 17.48 64.70 17.82
15–2 16.49 61.70 21.81 quently makes the UV aging depth in asphalt binder gradually
15–3 16.05 61.70 22.25 expand downwards with the increment of UV aging time. The exis-
tence of vertical gradient of molecular size distributions in asphalt
film, as shown in Table 2, can give an evidence to support the dif-
fusion hypothesis proposed by Zeng et al.
Fig. 12. The results of FTIR spectra of different layers in 15-day UV aged asphalt In order to describe the downward diffusion phenomenon of UV
sample. aged asphalt molecules more objectively, the fluorescence test is
Fig. 13. The results of functional group index of different layers in 15-day UV aged asphalt sample: (a) sulfoxide index, and (b) carbonyl index.
8 Z. Chen et al. / Construction and Building Materials 246 (2020) 118501
Fig. 14. The results of fluorescence test in different asphalt layers of control sample and 15-day UV aged sample.
designed and detailed in Section 2.7. The results of fluorescence There are also content gradients of oxidation products in UV
test in different asphalt layers of control sample and 15-day UV aged asphalt film, indicating disparities of aging degree in dif-
aged sample are shown in Fig. 14. As for control sample, the fluo- ferent asphalt layers.
rescence reaction is not observed in the middle and bottom asphalt The observation of inorganic fluorescent powders being able to
layers, except for the top asphalt layer. This indicates that inor- permeate into fresh asphalt film in lower layers by fluorescence
ganic fluorescent powders cannot diffuse downwards into lower microscope objectively demonstrates the ‘‘diffusion aging
asphalt layers without UV radiation influence. By contrast, the flu- model”.
orescence reaction is observed in both the middle and bottom
asphalt layers for 15-day UV aged sample, which verifies inorganic 5. Recommendations for future work
fluorescent powders can permeate into fresh asphalt film in lower
layers with the downward diffusion of UV aged asphalt molecules. This paper only considered the UV aging gradient phenomenon
The demonstrated ‘‘diffusion aging model” can in turn well explain under the pure UV aging. In future work, we will investigate the UV
why there are vertical gradients of rheological, molecular sizes and aging gradient in short-term aged asphalt binders, and evaluate the
chemical properties in asphalt film after a certain UV aging period. effects of thermal aging on UV aging gradient by comparing the dif-
ferences in results of aging gradient between the pure UV aging
4. Conclusions and the joint action of both UV and thermal aging. In addition,
because there are differences between outdoor natural weathering
In this paper, the phenomenon of ultraviolet radiation aging aging and indoor UV aging simulations, it is necessary to further
gradient in asphalt film with 3 mm thickness was investigated investigate the gradient phenomenon under natural weathering
by rheological properties, molecular size distributions, chemical aging influences. Further, the phenomenon of aging gradient in
functional groups contents and fluorescence tests. The detailed asphalt mixtures also needs to be investigated in future work.
conclusions can be drawn as follows:
CRediT authorship contribution statement
By complex modulus, phase angle, ZSV, Jnr, DSRFn and xc
indexes, it can be concluded that the effect of 6-day UV aging Zihao Chen: Data curation, Writing - original draft. Henglong
is almost negligible, but the UV aging depth can exceed 1 mm Zhang: Data curation, Writing - original draft. Haihui Duan: Data
after 9-day UV aging period and further exceed 2 mm after curation, Writing - original draft.
15-day UV aging period.
The GPC results indicate that a vertical gradient of molecular Declaration of Competing Interest
sizes tends to form in asphalt film during UV aging process.
Along the depth in asphalt film, the proportion of large mole- The authors declare that they have no known competing finan-
cules gradually declines while the proportion of small mole- cial interests or personal relationships that could have appeared
cules increases. to influence the work reported in this paper.
Z. Chen et al. / Construction and Building Materials 246 (2020) 118501 9
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